Thermal interface pastes nanostructured for high performance
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Thermal interface materials in the form of pastes are needed to improve thermal contacts, such as that between a microprocessor and a heat sink of a computer. High-performance and low-cost thermal pastes have been developed in this dissertation by using polyol esters as the vehicle and various nanoscale solid components. The proportion of a solid component needs to be optimized, as an excessive amount degrades the performance, due to the increase in the bond line thickness. The optimum solid volume fraction tends to be lower when the mating surfaces are smoother, and higher when the thermal conductivity is higher. Both a low bond line thickness and a high thermal conductivity help the performance. When the surfaces are smooth, a low bond line thickness can be even more important than a high thermal conductivity, as shown by the outstanding performance of the nanoclay paste of low thermal conductivity in the smooth case (0.009 μm), with the bond line thickness less than 1 μm, as enabled by low storage modulus G ', low loss modulus G " and high tan δ. However, for rough surfaces, the thermal conductivity is important. The rheology affects the bond line thickness, but it does not correlate well with the performance. This study found that the structure of carbon black is an important parameter that governs the effectiveness of a carbon black for use in a thermal paste. By using a carbon black with a lower structure (i.e., a lower DBP value), a thermal paste that is more effective than the previously reported carbon black paste was obtained. Graphite nanoplatelet (GNP) was found to be comparable in effectiveness to carbon black (CB) pastes for rough surfaces, but it is less effective for smooth surfaces. At the same filler volume fraction, GNP gives higher thermal conductivity than carbon black paste. At the same pressure, GNP gives higher bond line thickness than CB (Tokai or Cabot). The effectiveness of GNP is limited, due to the high bond line thickness. A thermal paste that is particularly effective for smooth surfaces was obtained by using nanoclay platelets (obtained by organic modification and subsequent chemical exfoliation) as the solid component. The superiority of the nanoclay paste for smooth surfaces is attributed to the submicrometer bond line thickness. Electrically nonconductive high-performance thermal paste was obtained by using either fumed alumina or fumed zinc oxide. The nonconductivity serves to avoid short circuiting in the electronic application environment. The fumed oxides are as effective as carbon black, but are advantageous in their electrical nonconductivity. Without fuming, the oxides are less effective. The silane coating on fumed metal oxides helps. Electrically nonconductive thermal pastes have also been attained using carbon as the thermally conductive solid component. Either fumed alumina or nanoclay is used to break the electrical connectivity of the carbon in the paste to obtain electrical nonconductivity. Among the nanostrucutred pastes developed in this dissertation research, the nanoclay (0.6 vol.%) paste is recommended for smooth surfaces. With the overall performance for smooth and rough surfaces considered, the carbon black (Tokai, 15 vol.%) paste is recommended. Carbon black (Tokai) is more effective than carbon black (Cabot), due to its small aggregate size. All the pastes developed are much more effective than carbon nanotube arrays investigated by others. The rheological behavior of the thermal pastes was studied under strain sweep, frequency sweep, steady state flow and temperature ramping. In the absence of a solid component, the vehicle is Newtonian and fluid-like. In the presence of a solid component, the paste is a Bingham plastic that exhibits shear thinning and mainly solid-like behavior. The addition of antioxidants enhances the solid-like character, increases the yield stress, the plastic viscosity and the bond line thickness, and decreases the thermal contact conductance. Double yielding behavior was observed in the CB(Cabot) and CB(Tokai) pastes, but not in the nanoclay and fumed alumina pastes. The plastic viscosity after complete yielding is higher when the solid volume fraction is higher. Upon heating from 25 to 120°C in the absence of antioxidants, G ' and the viscosity increase, while G " decreases, due to slight phase separation. The antioxidants reduce the phase separation tendency, so that G', G" and the viscosity do not change upon heating from 50 to 120°C. Upon heating from 25 to 50°C, all of G', G" and the viscosity decrease in the presence of antioxidants, due to increasing fluidity.